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JOURNAL OF HAZARDOUS MATERIALS · 2020 · IF 9.038

Highly efficient adsorption and immobilization of U(VI) from aqueous solution by alkalized MXene-supported nanoscale zero-valent iron

Siyi Wang,Lin Wang,Zijie Li,Pengcheng Zhang,Ke Du,Liyong Yuan,Shunyan Ning,Yuezhou Wei,Weiqun Shi

A novel composite of zero-valent iron nanoparticles supported on alkalized Ti 3 C 2 T x nanoflakes (nZVI/Alk-Ti 3 C 2 T x ) was constructed by an in-situ growth method for simultaneous adsorption and reduction U(VI) from aqueous solution in anoxic conditions . The effect of various factors such as adsorbent dose, pH, ionic strength, contact time, initial U(VI) concentration and environmental media were comprehensively investigated by batch experiments. Benefiting from the good dispersion uniformity of nZVI on MXene substrates, nZVI/Alk-Ti 3 C 2 T x exhibited rapid removal kinetics, excellent selectivity , 100% removal efficiency and up to 1315 mg g −1 uptake capacity for U(VI) capture. In the presence of mimic groundwater, 1.0 mM NaHCO 3 and 10 mg L −1 humic acid , the removal percentages of U(VI) by the composites could reach 95.1%, 88.9% and 69.5%, respectively. The reaction mechanism between U(VI) and nZVI/Alk-Ti 3 C 2 T x has been clarified based on FTIR , XANES , XPS and XRD analysis. Depending on the consumption of reactive nZVI in the composites and the solution pH, the elimination of U(VI) could be realized by different pathways including reductive immobilization in the form of UO 2 , inner-sphere surface complexation and hydrolysis precipitation. The present study illustrates that the nZVI/Alk-Ti 3 C 2 T x composite may be an efficient scavenger for radioactive wastewater purification in environmental remediation.

研究领域: 环境科学 · 材料科学
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2024 · IF 7.7

Effects of Fe(II) and humic acid on U(VI) mobilization onto oxidized carbon nanofibers derived from the pyrolysis of bacterial cellulose

Weisheng Dai,Yao Wang,Weijuan Guo,Guofu Wang,Muqing Qiu

The effects of Fe(II) and humic acid on U(VI) immobilization onto oxidized carbon nanofibers (Ox-CNFs, pyrolysis of bacterial cellulose) were investigated by batch, spectroscopic and modeling techniques, with results suggesting that, Ox-CNFs exhibited fast adsorption rate (adsorption equilibrium within 3 h), high adsorption performance (maximum adsorption capacity of 208.4 mg/g), good recyclability (no notable change after five regenerations) in the presence of Fe(II) towards U(VI) from aqueous solutions (e.g., 40 % reduction and 10 % adsorption at pH 8.0), which was attributed to the various oxygen-containing functional groups, excellent chemical stability, large specific surface area and high redox effect. U(VI) adsorption increased with increasing pH from 2.0 to 5.0, then high-level plateau and remarkable decrease were observed at 5.0–6.0 and at pH > 6.0, respectively. According to FT-IR and XPS analysis, a negative correlation between U(VI) reduction and organic in the presence of Fe(II) implied that U(VI) reduction was driven by Fe(II) while inhibited by humic acid. The interaction mechanism of U(VI) on Ox-CNFs was demonstrated to be adsorption and ion exchange at low pH and reduction at high pH according to XPS and surface complexation modeling. These findings filled the knowledge gaps pertaining to the effect of Fe(II) on the transformation and fate of U(VI) in the actual environment. This carbon material with distinctive performance and unique topology offers a potential platform for actual application in environmental remediation.

研究领域: 环境科学 · 材料科学
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Journal of Environmental Chemical Engineering · 2024 · IF 7.4

Enhanced removal of aqueous uranium: Photocatalytic U(VI) reduction over bismuth vanadate/hydrothermal carbon nitride under visible light

Jialin Qiu,Ye’an Zhu,Bo Wang,Yidan Nie,Zengkai Song,Peng Li,Zongbo Xie,Zhanggao Le

Photocatalytic removal of hexavalent uranium is an effective method for reducing radioactive uranium contamination in water. Herein, novel heterojunction catalysts, bismuth vanadate/hydrothermal carbon nitride (BiVO 4 /HCN), were synthesized and firstly successfully implemented for uranium removal. For example, the removal rate of U(VI) over 0.10BiVO 4 /HCN reached 98.5 % for the first time and more than 95.9 % for five consecutive cycles. Subsequent characterization analyzes confirmed that increased specific surface area, redshift of the absorption band, and efficient charge separation of the photogenerated electron-hole pairs collectively contributed to the improved photocatalytic performance. Noteworthily, free radical quenching and electron spin resonance spectroscopy results indicate that holes, photogenerated electrons, and superoxide radicals are the major active species for the photoreduction of U(VI). Finally, a possible photocatalytic mechanism of U(VI) removal was proposed.

CAS / MDL: 7803-55-6
研究领域: 环境科学 · 材料科学
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY · 2020 ·Vol. 324 ·期 2 ·813-822 · IF 1.137

Adsorption performance of U(VI) by amidoxime-based activated carbon

Liu Peng,Yu Qiang,Xue Yun,Chen Jiaqi,Ma Fuqiu

We present a simple strategy for preparing amidoxime modified activated carbon. The composition and morphology of the materials have been confirmed via powder XRD, BET, TGA, SEM and FT-IR studies. Batch adsorption experiment were exploited to explore adsorption performance of U(VI) by amidoxime-based activated carbon. The adsorption capacity of activated carbon was significantly improved after the modification by amidoxime, the amidoxime-based activated carbon was a possible adsorbent for adsorbing U(VI). This study reveals that with a facile synthesis and low-cost, amidoxime-based activated carbon can be regarded as a promising material for uranium-containing wastewater treatment.

CAS / MDL: 1668-00-4
研究领域: 环境科学 · 材料科学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2022 · IF 24.319

Photochemically triggered self-extraction of uranium from aqueous solution under ambient conditions

Yezi Hu,Duoyue Tang,Zewen Shen,Ling Yao,Guixia Zhao,Xiangke Wang

Photocatalytic extraction of uranium from nuclear wastewater and seawater is a highly promising strategy to avoid environmental pollution and effectively recover uranium resources. Herein, we propose a novel strategy of photochemical for efficiently and high selectively extracting uranium from aqueous solution. The excited UO 2 2+ at a suitable pH range were utilized for initiating the formation of hydrogen peroxide, which then directly reacted with UO 2 2+ to form solid studtite (UO 2 )O 2 ∙4 H 2 O. This photochemically triggered extraction approach could remove ∼100.0% of UO 2 2+ from aqueous solution with U(VI) concentration of 10.0–200.0 ppm, and 62.7% of UO 2 2+ from U(VI)-spiked real seawater after 24 hrs-irradiation under visible light even without additional electron-donor agents. The highly selective and high extraction efficiency towards uranium ranged in extremely wide concentrations demonstrated the powerful application potential in both the removal of uranium from nuclear wastewater and the extraction of uranium from seawater. Data Availability Data will be made available on request.

研究领域: 环境科学 · 材料科学
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JOURNAL OF MOLECULAR LIQUIDS · 2019 · IF 4.561

Mutual effect of U(VI) and phosphate on the reactivity of nanoscale zero-valent iron (nZVI) for their co-removal

Huiling Zheng,Xuemei Ren,Xiaodong Zhang,Gang Song,Diyun Chen,Changlun Chen

Nanoscale zero-valent iron (nZVI) has been widely considered as a promising permeable barrier material for remediating U(VI)-contaminated waters. Little information is available regarding co-removal of U(VI) and oxyanion contaminants by nZVI, yet in the majority of areas polluted by U(VI), co-existence of phosphate is found to be common especially in eutrophic water. Herein, the mutual influence of U(VI) and phosphate on the effectiveness of nZVI in co-removing U(VI) and phosphate is investigated by macroscopic and microscopic approach. The results indicate that nZVI can effectively co-remove U(VI) and phosphate and the processes intensively depend on the solution pH and the additional order due to the formation of nZVI-U(VI)-phosphate complexes and will change the morphology of nZVI through the formation of a new phase. Furthermore, the maximum removal capacity of nZVI increases by 21.63% at pH 6.0 for U(VI) ions and by 34.28% at pH 7.0 for phosphate when both U(VI) and phosphate are present simultaneously. In short, the co-presence of U(VI) and phosphate has a great impact on the reactivity and morphology of nZVI. The findings will be beneficial to broaden the potential feasibility of nZVI in simultaneous radionuclide and phosphate pollution cleanup.

研究领域: 环境科学 · 放射生物学
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SCIENCE OF THE TOTAL ENVIRONMENT · 2019 · IF 5.589

Porous biochar modified with polyethyleneimine (PEI) for effective enrichment of U(VI) in aqueous solution

Xin Wang,Jinghua Feng,Yawen Cai,Ming Fang,Mingguang Kong,Ahmed Alsaedi,Tasawar Hayat,Xiaoli Tan

This study investigated the modification of moso bamboo biochar with polyethyleneimine (PEI) for the efficient enrichment of U(VI) in aqueous solution. The alkali/acid treated biochars with amine groups (PEI-alkali-biochar or PEI-acid-biochar) were characterized by SEM , BET, TGA , FTIR and XPS. The effects of contact time, U(VI) concentration, pH and ionic strength on U(VI) adsorption by PEI-alkali/acid-biochar were studied. U(VI) adsorption process on PEI-alkali/acid-biochar obeys pseudo-second-order model. Intraparticle diffusion model was used to investigate the controlled factors of the adsorption process. The fitting of Langmuir model gives the maximum adsorption capacities of 212.7 mg/g for PEI-alkali-biochar and 185.6 mg/g for PEI-acid-biochar, which are almost 9–10 times higher than that of pristine biochar (20.1 mg/g). The thermodynamic parameters illustrate that U(VI) adsorption on PEI-alkali/acid-biochar is an exothermic and spontaneous process. The FTIR and XPS analyses imply that U(VI) adsorption by PEI-alkali/acid-biochar is mainly controlled by complexation between U(VI) and amine groups. PEI-alkali/acid-biochar could be considered as a low-cost and outstanding material for U(VI) removal from radionuclide wastewater in practical application.

CAS / MDL: 9002-98-6
研究领域: 环境科学 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Self-oxidation cycle of oxidized red phosphorus for regeneration of binding sites enables efficient uranium extraction in tributylphosphate-kerosene system

Yingtong Lv,Ru Cheng,Guolin Yang,Wang Liu,Jingye Zhang,Xiaofang Yu,Wencai Bai,Rong He,Wenkun Zhu

Photocatalytic extraction of hexavalent uranium (U(VI)) is challenging in organic phase, especially the widely used tributylphosphate (TBP)-kerosene system in the nuclear fuel cycle process. Organic components in TBP-kerosene system are difficult to be oxidized, which limits the reduction of U(VI). Herein, we demonstrated a self-oxidation strategy to enable the photocatalytic cycle of U(VI) reduction in TBP-kerosene system by the deeply oxidized commercial red phosphorus (DO-CRP). In the 30 %TBP-kerosene solution, the DO-CRP exhibited 88.0 % of extraction efficiency with 580.8 mg/g of capacity for U(VI) within 120 min. In this process, PO 4 3− groups generated at the defects were used as the binding sites to capture and reduce U(VI). Following desorption process involved in the cleavage of uranium and PO 4 3− groups, which released defect sites for self-oxidation in the next cycle. Mechanistic study revealed that such regeneration of self-oxidation and U(VI) binding sites achieved the continuous photocatalytic extraction of U(VI) in TBP-kerosene system.

CAS / MDL: 7723-14-0 497-19-8
研究领域: 化学工程 · 核能科学
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Is the sacrificial agent really just a sacrificial agent? A case study on the photocatalytic reduction of U(VI) by alcohols

Si-Yu Chen,Ji-Pan Yu,Zhi-Fang Chai,Wei-Qun Shi,Li-Yong Yuan

Although organic sacrificial agents are often used to improve the efficiency of photocatalytic reactions, the impact of their existence on the performance evaluation of photocatalysts has not been analyzed yet. In this study, to clearly understand the role of organic sacrificial agents in the photocatalytic process, the photocatalytic reduction of hexavalent uranium (U(VI)) by alcohols is systematically analyzed. The results reveal that under the conditions of pH 5, nitrogen atmosphere, visible light irradiation, and no photocatalyst, the alcohol sacrificial agents can directly reduce U(VI) with efficiencies as high as 98%. Uranium dioxide, formaldehyde, and hydrogen ion are identified as the final products of the photocatalytic reaction, and the reaction mechanism is proposed based on the results of electron paramagnetic resonance (EPR) spectroscopy. Accordingly, it is inferred that alcohol as an organic sacrificial agent markedly interferes with the performance evaluation of photocatalysts during the photocatalytic reduction of U(VI). Overall, this study provides valuable insights into the actual role of sacrificial agents in the photocatalytic reduction process.

研究领域: 环境科学 · 化学
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CHEMICAL ENGINEERING JOURNAL · 2019 · IF 8.355

Adsorptive and reductive removal of U(VI) by Dictyophora indusiate-derived biochar supported sulfide NZVI from wastewater

Hongwei Pang,Zhuofan Diao,Xiangxue Wang,Yan Ma,Shujun Yu,Hongtao Zhu,Zhongshan Chen,Baowei Hu,Jianrong Chen,Xiangke Wang

Nanoscale zero-valent iron (NZVI) has been considered as a potential scavenger for U(VI) elimination from aqueous environment. To decrease the aggregation and to improve antioxidation, sulfidation technology and biochar were applied to modify NZVI. In this work, Dictyophora indusiate -derived biochar supported sulfide NZVI (DI-SNZVI) was synthesized and applied for U(VI) elimination. The excellent behaviors of kinetics (3 h for equilibrium), thermodynamic research and maximum removal amounts (427.9 mg·g −1 at pH = 5.0 and 298 K) revealed the outstanding performances of DI-SNZVI in U(VI) removal. The cycle experiments and different water system investigations further illustrated its potential ability for real applications. Moreover, the abundant functional groups and FeS x shell of DI-SNZVI were proved to be responsible for the enhanced removal of U(VI). In the end, the macroscopic and XPS study revealed that U(VI) elimination mechanisms were synergistic attributed to the adsorptive and reductive processes. This paper highlighted the biochar-based sulfide NZVI for efficient U(VI) elimination in environmental pollution management.

研究领域: 环境科学 · 材料科学
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Environmental Science-Nano · 2018 ·Vol. 5 ·期 7 ·1584-1594 · IF 6.087

Phosphatidyl-assisted fabrication of graphene oxide nanosheets with multiple active sites for uranium(VI) capture

Peipei Yang,Qi Liu,Hongsen Zhang,Jingyuan Liu,Rongrong Chen,Rumin Li,Di Wu,Xuefeng Bai,Jun Wang

A novel kind of graphene oxide-based (GO-based) adsorbent was successfully prepared by chemical modification with cetyltrimethylammonium bromide (C16TAB) and phytic acid (PA) for adsorbing uranium (U(VI)). A close relationship between PA and GO interlayer spacing was investigated; the optimal spacing was 3.88 Å with 4.5 mL PA. A series of adsorption experiments were carried out with the as-prepared product (denoted as GO–C16TAB–PA) to capture U(VI) ions. The adsorption capacity of the GO–C16TAB–PA adsorbent can reach 923 mg g−1 (298.15 K) with an excellent removal rate (∼90%), which demonstrates a 527% increment compared with that of pristine GO in the same environment (pH = 8, Co = 500 mg L−1). Meanwhile, the adsorption equilibrium time of GO–C16TAB–PA was shortened by 50% compared with that of pristine GO. In addition, the GO–C16TAB–PA adsorbent exhibited superior recyclability with a six-adsorption–desorption-cycle test. Finally, the fabricated GO–C16TAB–PA adsorbent exhibited excellent adsorption performance in simulated seawater, providing a theoretical guide and methodology for further seawater extraction of uranium(VI).

研究领域: 环境科学 · 材料科学
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SCIENCE OF THE TOTAL ENVIRONMENT · 2022 · IF 10.753

Bismuth impregnated biochar for efficient uranium removal from solution: Adsorption behavior and interfacial mechanism

Jun Liao,Xiaoshan He,Yong Zhang,Wenkun Zhu,Lin Zhang,Zhibing He

In this work, Bi 2 O 3 doped horse manure-derived biochar was obtained by carbonizing the H 2 O 2 -modified horse manure loaded with bismuth nitrate under nitrogen atmosphere at 500 °C. The results showed that there was a sharp response between the as-prepared bismuth impregnated biochar and uranium(VI) species in solution, which resulted in a short equilibrium time (<80 min), a fast adsorption rate (about 5.0 mg/(g·min)), a high removal efficiency (93.9%) and a large adsorption capacity (516.5 mg/g) ( T  = 298 K, pH = 4, C i  = 10 mg/L and m/V = 0.1 g/L). Besides, the removal behavior of the bismuth impregnated biochar for uranium(VI) did not depend on the interfering ions and ion strength, except Al 3+ , Ca 2+ , CO 3 2− and PO 4 3− . These results indicated that the modified biochar might possess the potential of remediating the actual uranium(VI)-containing wastewater. Moreover, the interaction mechanism between Bi 2 O 3 doped biochar and uranium(VI) species was further explored. The results demonstrated that the enrichment of uranium(VI) on the surface of the as-prepared biochar was controlled by various factors, such as surface complexation, ion exchange, electrostatic attraction, precipitation and reduction, which facilitated the adsorption of uranium(VI) on the bismuth impregnated biochar.

研究领域: 环境科学 · 材料科学
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